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Multiscale Structural Characterization of Biobased Diallyl–Eugenol Polymer Networks

Abstract : Biosourced eugenol-based polymer networks have a potential functionality for antibacterial coating applications. The presence of carvacrol, a phenol compound, exacerbates these properties. However, the relationship between the network structure and the macroscopic thermomechanical behavior is not known for these biopolymers. Thus, this work details a robust study of this relationship through a multiscale experimental approach combining Dielectric spectroscopy, DMA, Tensile testing and Time domain DQ 1 H NMR. It was shown that carvacrol has an influence on the molecular mobility of the materials. Namely it induces the appearance of a shouldering on the γ relaxation and a diminishing of T α. More surprisingly, up to 20% wt , carvacrol increases the elastic E and Young's E moduli. This observation can be interpreted as an increase of the crosslink density ν C of the networks. Time domain DQ 1 H NMR shows that the 1 residual dipolar coupling constant D res also increases. Thus, carvacrol seems to act as both a thermal plasticizer and a mechanical reinforcement, which may seem to be antagonistic trends. For carvacrol contents over 20% wt these properties diminish due to a saturation of this molecule in the networks and the onset of a phase separation. By combining the aforementioned techniques, it was proven that carvacrol linearly increased the measured crosslink density and thermomechanical properties by physically bonding to the networks through π − π interactions. These interactions would act as physical crosslinks. This work demonstrates that by correlating the results of various multiscale experimental techniques, a better comprehension of the structure-property relationship can be established for biobased functional polymer networks.
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https://hal.archives-ouvertes.fr/hal-03010531
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Submitted on : Monday, November 23, 2020 - 5:04:08 PM
Last modification on : Wednesday, March 16, 2022 - 3:54:01 AM
Long-term archiving on: : Thursday, February 25, 2021 - 1:37:14 PM

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Agustín Rios de Anda, Paul Sotta, Tina Modjinou, Valérie Langlois, Davy-Louis Versace, et al.. Multiscale Structural Characterization of Biobased Diallyl–Eugenol Polymer Networks. Macromolecules, American Chemical Society, 2020, 53 (6), pp.2187-2197. ⟨10.1021/acs.macromol.9b02280⟩. ⟨hal-03010531⟩

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